Method of providing a nuclear fuel and a fuel element provided by such a method

ABSTRACT

A nuclear fuel element including a uranium-molybdenum alloy that provides an enhanced reactivity in research, test and radioisotope production nuclear reactors. In this uranium-molybdenum alloy, the uranium is enriched in the isotope 235-U, while the molybdenum is depleted in the isotope 95-Mo. The thus obtained enhanced reactivity provides, depending on the exact use of the fuel element, a requirement for less uranium in the fuel and the use of the fuel elements during a longer period in the reactor.

CROSS REFERENCE TO RELATED APPLICATIONS

This application is a divisional of U.S. application Ser. No.10/383,861, filed Mar. 10, 2003 now U.S. Pat. No. 7,187,744, whichclaimed priority to European Application 02075937.9, filed Mar. 11,2002, the entire contents of both applications being incorporated hereinby reference.

BACKGROUND OF THE INVENTION

1. Field of the Invention

This invention relates to a method for providing a nuclear fuel and afuel element provided with a nuclear fuel made by such a method.

2. Description of the Related Art

It is known to produce nuclear fuels containing relatively low densitiesof highly enriched uranium. Highly enriched uranium (HEU) has thedisadvantage that for political reasons, the use of this material isundesirable, because it can not only be deployed for peaceful purposesbut can also be used for less peaceful applications, as for perpetratingterrorist attacks and/or manufacturing atomic bombs. For this reason inrecent years the use of low enriched uranium (LEU), which has a 235-Ucontent of less than 20%, is strongly encouraged. In view of theabove-mentioned disadvantage of HEU, a nuclear fuel preferably comprisesuranium not highly enriched in the 235-U isotope. A disadvantage of sucha fuel, however, is that the total uranium content (the sum of allisotopes) in an LEU-containing fuel element must be much higher thanthat in an HEU-containing fuel element, in order to obtain a similarreactivity. However, metallic uranium inherently has insufficientmechanical stability during irradiation to be used in elemental form.

It is known to impart stability to the uranium by using it in a chemicalcomposition with silicon, e.g. U₃Si₂. In this composition, however, thedensity of the uranium still cannot always attain the desired highervalue to be able to provide a reactivity sufficiently high to enhancethe utility or the economics of the reactor. For this reason a new classof nuclear fuels for use in research, test and radioisotope-productionreactors is being developed based on uranium-molybdenum alloys. The highuranium density of these alloys should make it possible to fuel thesereactors using LEU instead of HEU, without causing a large decrease ofthe neutron flux in these reactors. These uranium-molybdenum alloysoffer the further advantage of being able to be reprocessed in currentlyoperating reprocessing plants.

Uranium-molybdenum alloys are currently being tested as dispersions ofalloy fuel particles in a non-fissionable matrix material, such asaluminum, and as a monolithic fuel. Both types of fuel are enclosed in acladding such as aluminum. U.S. Pat. No. 5,978,432 describes one methodof producing a dispersion fuel using uranium-molybdenum alloys. The mostcommon design of a Material Test Reactor (MTR) fuel element using U-Mofuel and U-Mo fuel plates is as follows. U-Mo particles are dispersedinto an aluminum matrix. The dispersed particles and the aluminum matrixmake up a thin fuel layer, which is placed between two thin claddingplates of aluminum alloy. Such a cladding is, for example, described inthe U.S. Pat. No. 4,963,317. In the present invention, the aluminummatrix is to be understood to comprise the aluminum of the fuel only.Therefore, the bulk of the aluminum cladding does not form part of thematrix in the present invention.

The thus-obtained fuel plates, each comprising a fuel layer enclosed bycladding plates, are either curved or flat. Approximately 20 of suchplates form a fuel element together with structural components. Coolingwater that flows between the plates cools the fuel plates fuelling areactor during the operation thereof.

Although the use of uranium-molybdenum alloys makes it possible toincrease the uranium density in the nuclear fuel for research and testreactors, the use of molybdenum carries the penalty of a significantneutron absorption, which decreases the effect of the added uranium,resulting in a relatively low reactivity. Therefore, the application ofmolybdenum in a nuclear fuel has been unfavourable albeit itsadvantages.

SUMMARY OF THE INVENTION

It is an aspect of the present invention to overcome the problemsdescribed above of providing a nuclear fuel that comprises anuranium-molybdenum alloy, in particular it is an aspect of the presentinvention to increase the reactivity of such a fuel.

To that end, the present invention provides a nuclear fuel including analloy of metallic uranium and molybdenum, the uranium being enriched inthe isotope 235-U, while the molybdenum is depleted in the isotope95-Mo.

The present invention is based on Applicant's discovery that the use ofmolybdenum depleted in 95-Mo, which absorbs less neutrons compared tonatural molybdenum, results in a higher reactivity of the nuclear fuel.This effect is explained below. The higher reactivity can be used torender a number of advantages, depending among others on the specificdesign of the fuel element to be used and the manner in which the fuelelement is used. Possible advantages of using molybdenum depleted in95-Mo are: high reactivity; increased flux; achieving a higherconcentration of molybdenum in the fuel in case of 95-Mo-depletedmolybdenum, while retaining identical flux, which may render anincreasingly stable fuel; identical flux, but with a longer cycle, whichallows for consumption of a smaller quantity of fuel elements; and/orsmaller quantity of expensive enriched uranium per fuel element toretain identical flux.

DETAILED DESCRIPTION

The reasons for the effect of the use of molybdenum depleted in 95-Moinstead of natural molybdenum, are shown in Table 1 below, whichincludes the thermal neutron absorption cross section (D) and theresonance integral of various molybdenum isotopes. The thermal neutronabsorption cross section and the resonance integral are measures for theamount of thermal neutrons and epi-thermal neutrons absorbed by themolybdenum respectively. The thermal neutron cross section data in Table1 originate from the 81^(St) edition of the Handbook of Chemistry andPhysics (2000-2001), CRC Press, Robert C. Weast et al, page 11-165/166.The resonance integral data are a typical example of the results ofneutronics computations.

TABLE 1 Effective cross section of molybdenum isotopes for neutrons. Thevalues for natural Mo have been computed using the weighed averages ofthe data for the isotopes. Molybdenum Abundant Resonance isotope atomic% D (barns) Integral (barns) 92-Mo 14.84 0.06 0.8 94-Mo  9.25 0.02 0.895-Mo 15.92 13.4 109 96-Mo 16.68 1.5 17 97-Mo  9.55 2.2 14 98-Mo 24.130.14 7.2 100-Mo   9.63 0.19 3.6 Natural Mo — 2.7 23.8

Table 1 shows that 95-Mo has both the highest thermal neutron absorptioncross section (D) and the highest resonance integral. Therefore thepresence of the considerable fraction 95-Mo in natural molybdenum (about16%) has a significant negative impact on the reactivity of U-Mo fuelcontaining natural Mo. Comparing the computed D-value and the computedresonance integral for natural molybdenum with those for the isotopes92-Mo, 94-Mo, 96-Mo, 97-Mo, 98-Mo and 100-Mo shows that all theseisotopes have a lower computed D-value and a lower computed resonanceintegral compared to natural molybdenum. This shows that the use of allthese isotopes will increase the reactivity compared to the use ofnatural molybdenum. The data in Table 1 show that 92-Mo and 94-Mo havethe lowest values for the thermal neutron absorption cross section (D)and the resonance integral of all molybdenum isotopes. The data in Table1 show that 96-Mo and 97-Mo have values for the thermal neutronabsorption cross section (D) and the resonance integral which are onlysomewhat lower than those for natural molybdenum. The data in Table 1show that 98-Mo and 100-Mo have values for the thermal neutronabsorption cross section (D) and the resonance integral which areintermediate between those of 92-Mo and 94-Mo on the one hand and 96-Moand 97-Mo on the other hand. The isotopic composition that will beapplied in practical applications will depend on various parameters,such as the costs of enrichment of the molybdenum in 92-Mo and 94-Mocompared to the costs of enrichment of the molybdenum in 98-Mo and100-Mo.

The impact of the use of molybdenum depleted in 95-Mo in U-Mo fuel in atest reactor can lead to an annual savings of 2.5 to 3 fuel elements.This means that fewer fuel elements must be purchased at high cost andfewer spent fuel elements must be disposed of at even higher cost.

The production of molybdenum which does not contain any 95-Mo is notfeasible from a technical point of view. Therefore, the 95-Mo-depletedmolybdenum will still contain some 95-Mo. The 95-Mo concentration thatwill be used for practical application will depend on variousparameters, such as: the costs of the enrichment of uranium in 235-U andthe costs of depletion of molybdenum in 95-Mo; the costs for theproduction of fuel plates and fuel elements; and/or the costs ofdisposing of spent fuel elements.

According to a further embodiment of the present invention, the depletedmolybdenum contains less than 15% by weight, more particularlyapproximately 5% by weight, of the molybdenum isotope 95-Mo. With thesepercentages by weight of the molybdenum isotope 95-Mo, relatively highreactivity values are obtained.

According to an even further embodiment of the present invention, thecontent of molybdenum in the uranium-molybdenum alloy is in the range of2-20% by weight, more particularly in the range of 5-10% by weight. Whenthe fuel contains such an amount of molybdenum, a relatively highconcentration of uranium can be incorporated therein without the uraniumbecoming mechanically unstable during irradiation. In particular, at acontent of 5-10% by weight, sufficient uranium can be present in thefuel to obtain a neutron yield useful for the purposes mentionedearlier. In a preferred embodiment, the fuel contains more than 3grams/cm³, more particularly more than 4 grams/cm³, of uranium. Morepreferably, the fuel contains more than 5 grams/cm³, more particularlymore than 7.5 grams/cm³, of uranium. Such densities of enriched uraniumprovide relatively high neutron yields and high reactivity values. Afuel that comprises uranium in such relatively high densities cancomprise an aluminum matrix embedding the alloy of uranium andmolybdenum, so that a stable fuel meat is formed.

The present invention further provides a fuel element. Such a nuclearfuel element can be made by a method according to the invention. Such afuel element is relatively simple to recycle, compared with, forinstance, fuel elements containing uranium-silicon compounds. Since thefuel element is not provided with highly enriched uranium, production,transport and use of such a fuel element is preferable, from anon-proliferation point of view, to fuel elements that do contain highlyenriched uranium.

The advantages discussed above of using molybdenum depleted in theisotope 95-Mo result for any level of uranium enrichment, although indifferent degree. Therefore, the present invention is applicable to alllevels of uranium enrichment. The enriched uranium can for examplecontain 2-40% by weight, in particular 10-20% by weight, of the isotope235-U. On the other hand, a fuel comprising an alloy of a higherenriched uranium, such as HEU, and Mo-95 depleted molybdenum is alsowithin the scope of the present invention. Enrichment of this uraniumcan be implemented in different ways, for example by utilizingultracentrifuges, by gas diffusion, or by a combination of these orother methods. Besides, the enriched uranium can be obtained from themixing of highly enriched uranium with lowly enriched or naturaluranium. This is also known as HEU downblending.

Further, the depleted molybdenum can have been obtained in differentways, for example by utilizing ultracentrifuges.

The molybdenum can also be enriched in the isotope 92-Mo, 94-Mo, 96-Mo,97 Mo, 98-Mo and/or 100-Mo, resulting in molybdenum which is effectivelydepleted in 95-Mo.

To those skilled in the art, it will be clear that various modificationsare possible within the scope of the present invention.

1. A fuel element for use in a nuclear reactor, comprising an alloy anda matrix with the alloy dispersed in the matrix, the alloy comprisinguranium enriched in isotope 235-U and processed molybdenum, wherein theprocessed molybdenum is depleted in isotope 95-Mo prior to formation ofthe fuel element such that the processed molybdenum absorbs lessneutrons compared to natural molybdenum, wherein the fuel element has ahigher reactivity than that of a comparative fuel element having a samecomposition as that of the fuel element except that unprocessed, naturalmolybdenum is substituted for the processed molybdenum.
 2. A fuelelement according to claim 1, wherein the matrix comprises aluminum. 3.A fuel element according to claim 1, wherein the processed molybdenumcontains less than 15% by weight of the isotope 95-Mo.
 4. A fuel elementaccording to claim 1, wherein the alloy contains the processedmolybdenum in a range of 2-20% by weight.
 5. A fuel element according toclaim 1, wherein the uranium contains 2-40% by weight of the isotope235-U.
 6. A fuel element according to claim 1, wherein the alloycontains more than 3 grams/cm³ of the uranium.
 7. A fuel elementcomprising uranium and processed molybdenum, the fuel element made by amethod comprising processing molybdenum to deplete isotope 95-Mo andform the processed molybdenum, and subsequently forming an alloy of ametallic uranium and the processed molybdenum dispersed in a matrix,wherein the uranium is enriched in isotope 235-U, wherein the fuelelement has a higher concentration of molybdenum isotopes than that in acomparative fuel element comprising unprocessed, natural molybdenum andhaving an identical flux as that of the fuel element.
 8. A fuel elementaccording to claim 7, wherein the alloy contains more than 3 grams/cm³of the uranium.
 9. A fuel element according to claim 7, wherein theprocessed molybdenum contains less than 15% by weight of the isotope95-Mo.
 10. A fuel element according to claim 7, wherein said processingmolybdenum comprises enriching molybdenum in isotopes 92-Mo, 94-Mo,96-Mo, 97-Mo, 98-Mo, 100-Mo, or any combination thereof.
 11. A fuelelement according to claim 7, wherein the alloy contains the processedmolybdenum in a range of 2-20% by weight.
 12. A fuel element accordingto claim 7, wherein the uranium contains 2-40% by weight of the isotope235-U.
 13. A fuel element according to claim 7, wherein the matrixcomprises aluminum.
 14. A fuel element according to claim 7, whereinsaid processing molybdenum comprises using an ultracentrifuge.
 15. Afuel element according to claim 1, wherein the processed molybdenumcontains less than 5% by weight of the isotope 95-Mo.
 16. A fuel elementaccording to claim 7, wherein the processed molybdenum contains lessthan 5% by weight of the isotope 95-Mo.
 17. A fuel element of claim 1,wherein the fuel element has a higher concentration of molybdenumisotopes than that in the comparative fuel element, wherein thecomparative fuel element has an identical flux as that of the fuelelement.
 18. A fuel element of claim 7, wherein the fuel element has ahigher reactivity than that of the comparative fuel element, wherein thecomparative fuel element has a same composition as that of the fuelelement except that the unprocessed, natural molybdenum is substitutedfor the processed molybdenum.